Photocatalytic degradation of tetrabromobisphenol A by mesoporous BiOBr: Efficacy, products and pathway

Photocatalytic degradation of tetrabromobisphenol A by mesoporous BiOBr: Efficacy, products and pathway
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DOI:
10.1016/j.apcatb.2011.07.036
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发表时间:
2011-09
影响因子:
22.1
通讯作者:
Jian Xu;W. Meng;Y. Zhang;Lei Li;Changsheng Guo
Jian Xu;W. Meng;Y. Zhang;Lei Li;Changsheng Guo
中科院分区:
化学1区
文献类型:
--
作者:
Jian Xu;W. Meng;Y. Zhang;Lei Li;Changsheng Guo

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四溴双酚A(TBBPA)是目前世界上使用最广泛的溴系阻燃剂。在本研究中,我们第一次探讨了TBBPA的光催化氧化的纳米结构的BiOBr微球。采用溶剂热法制备了BiOBr光催化剂,考察了不同制备条件下BiOBr光催化剂的表征结果和对罗丹明B(RhB)的去除效果,确定了最佳制备条件。所制备的BiOBr为纯四方晶相的介孔材料,模拟太阳光照射60 min后,对RhB的去除率接近100%。采用BiOBr降解TBBPA,在UV-vis/BiOBr体系中15 min后TBBPA几乎被完全去除。动力学分析表明,BiOBr和P25 TiO 2的反应速率常数分别为0.388和0.101 min − 1,表明BiOBr有效地促进了TBBPA的分解。通过HPLC-MS和HPLC-SIR-MS鉴定了8种主要的反应产物或中间体,并初步提出了TBBPA的降解途径。该机理初步阐明了羟基化和脱溴反应在TBBPA转化过程中起重要作用。介孔BiOBr在去除TBBPA方面的卓越效率代表了用于处理含TBBPA的废水或修复TBBPA污染的环境基质的有前途的技术。
Tetrabromobisphenol A (TBBPA) is the most widely used brominated flame retardant around the world. In the present study, for the first time we explored the photocatalytic oxidation of TBBPA by nanoarchitectural BiOBr microspheres. BiOBr photocatalysts were synthesized via solvothermal method with various preparation conditions, and the optimal synthesis condition was determined according to their characterization results and rhodamine B (RhB) removal efficiencies. The prepared optimal BiOBr was mesoporous material of pure tetragonal phase, which removed nearly 100% of RhB from solution after 60min simulated solar light irradiation. The BiOBr was adopted to decompose TBBPA, which was almost totally eliminated after 15min in the UV–vis/BiOBr system. The kinetic analysis indicated that the reaction rate constants were 0.388 and 0.101min−1for BiOBr and P25 TiO2, respectively, suggesting that BiOBr effectively and kinetically enhanced the decomposition of TBBPA. Eight major reaction products or intermediates were identified by HPLC–MS and HPLC–SIR–MS, and a tentative degradation pathway of TBBPA was proposed. The mechanism originally illustrated that both hydroxylation and debromination played important roles in TBBPA transformation. The exceptional efficiency of mesoporous BiOBr in removing TBBPA represents a promising technique for treatment of TBBPA-containing wastewater or remediation of TBBPA-contaminated environmental matrices.